Carbon nanoparticles were prepared by refluxing the combustion soot of natural gas in nitric acid. Transmission Electron Microscopy measurements showed that the resulting particles exhibited an average diameter of 4.8 ± 0.6 nm, and the crystalline lattices were consistent with graphitic carbons. 13C NMR and FTIR spectroscopic measurements further confirmed the presence of sp2 carbons in the form of aryl and carboxylic/carbonyl moieties. The resulting carbon nanoparticles were found to emit photoluminescence with a quantum yield of approximately 0.43%. Additionally, the emission band energy of the carbon nanoparticle was very similar to that of much smaller carbon nanoparticles obtained from candle soot, suggesting that the photoluminescence might arise from particle surface states, analogous to the behaviors of semiconductor quantum dots with an indirect bandgap. In electrochemical measurements, two pairs of well-defined voltammetric waves were observed, which might be ascribed to the peripheral functional moieties that were analogous to phenanthrenequinone derivatives. Interestingly, the carbon nanoparticles might also be exploited as nanoscale structural scaffolds for the deposition of nanostructures of varied transition metals, leading to the formation of metal−carbon functional nanocomposites.
An organic polymer nano-photocatalyst has been developed for highly efficient light driven proton reduction.
For the first time, organic semiconducting polymer dots (Pdots) based on poly[(9,9'-dioctylfluorenyl-2,7-diyl)-co-(1,4-benzo-{2,1',3} thiadiazole)] (PFBT) and polystyrene grafting with carboxyl-group-functionalized ethylene oxide (PS-PEG-COOH) are introduced as a photocatalyst towards visible-light-driven hydrogen generation in a completely organic solvent-free system. With these organic Pdots as the photocatalyst, an impressive initial rate constant of 8.3 mmol h(-1) g(-1) was obtained for visible-light-driven hydrogen production, which is 5-orders of magnitude higher than that of pristine PFBT polymer under the same catalytic conditions. Detailed kinetics studies suggest that the productive electron transfer quench of the excited state of Pdots by an electron donor is about 40 %. More importantly, we also found that the Pdots can tolerate oxygen during catalysis, which is crucial for further application of this material for light-driven water splitting.
Solution‐processed colloidal quantum dot (CQD) solar cells harvesting the infrared part of the solar spectrum are especially interesting for future use in semitransparent windows or multilayer solar cells. To improve the device power conversion efficiency (PCE) and stability of the solar cells, surface passivation of the quantum dots is vital in the research of CQD solar cells. Herein, inorganic CsPbI3 perovskite (CsPbI3‐P) coating on PbS CQDs with a low‐temperature, solution‐processed approach is reported. The PbS CQD solar cell with CsPbI3‐P coating gives a high PCE of 10.5% and exhibits remarkable stability both under long‐term constant illumination and storage under ambient conditions. Detailed characterization and analysis reveal improved passivation of the PbS CQDs with the CsPbI3‐P coating, and the results suggest that the lattice coherence between CsPbI3‐P and PbS results in epitaxial induced growth of the CsPbI3‐P coating. The improved passivation significantly diminishes the sub‐bandgap trap‐state assisted recombination, leading to improved charge collection and therefore higher photovoltaic performance. This work therefore provides important insight to improve the CQD passivation by coating with an inorganic perovskite ligand for photovoltaics or other optoelectronic applications.
Dendritic spines have been proposed to function as electrical compartments for the active processing of local synaptic signals. However, estimates of the resistance between the spine head and the parent dendrite suggest that compartmentalization is not tight enough to electrically decouple the synapse. Here we show in acute hippocampal slices that spine compartmentalization is initially very weak, but increases dramatically upon postsynaptic depolarization. Using NMDA receptors as voltage sensors, we provide evidence that spine necks not only regulate diffusional coupling between spines and dendrites, but also control local depolarization of the spine head. In spines with high-resistance necks, presynaptic activity alone was sufficient to trigger calcium influx through NMDA receptors and R-type calcium channels. We conclude that calcium influx into spines, a key trigger for synaptic plasticity, is dynamically regulated by spine neck plasticity through a process of electrical compartmentalization.
A facile room-temperature surfactant-free solution–chemical route has been developed to fabricate Cu2O nanocubes, octahedrons, spheres, plates, and polyhedrons by varying the reaction atmosphere (air or Ar) and reducing agent. It is believed that the oxygen adsorption and reaction on the surface of Cu2O may be able to slow down the reduction of Cu(OH)2 and the nucleation of Cu2O and further exert a noticeable influence on the following growth. We find that reducing agents are also important in determining the samples’ final morphology, structure, and composition. It has been demonstrated that the size of Cu2O nanocrystals can be modulated by changing the pH value of the reacting solution or the initial concentration of reacting agents or by adding solvents with high viscosity. In addition, the organic catalytic activity has been demonstrated to be susceptible to the shapes of the synthesized Cu2O materials. {111} planes of Cu2O are found to show higher catalytic activity (two times at 30 °C) than that of {100} facets on the N-arylation reaction of iodobenzene with imidazole. The difference among various crystal planes in catalytic activity may be related to crystal facets’ densities of surface Cu atoms, surface energies, turnover frequency, and electronic surface properties. Furthermore, O2-assisted selective etching is proposed to improve the activity of {100} facets by increasing the active sites. This fundamental understanding shows that morphological control of transition-metal oxides allows selective exposure of catalytically active planes and will most probably be applicable in the development of the next generation of highly efficient heterogeneous catalysts. The selective etching of crystallographic planes may be developed to a general technique to improve catalytic activity of noble metal, oxide nanocrystals, as well as porous catalysts.
Colloidal quantum dot (CQD) solar cells have high potential for realizing an efficient and lightweight energy supply for flexible or wearable electronic devices. To achieve highly efficient and flexible CQD solar cells, the electron transport layer (ETL), extracting electrons from the CQD solid layer, needs to be processed at a low-temperature and should also suppress interfacial recombination. Herein, a highly stable MgZnO nanocrystal (MZO-NC) layer is reported for efficient flexible PbS CQD solar cells. Solar cells fabricated with MZO-NC ETL give a high power conversion efficiency (PCE) of 10.4% and 9.4%, on glass and flexible plastic substrates, respectively. The reported flexible CQD solar cell has the record efficiency to date of flexible CQD solar cells. Detailed theoretical simulations and extensive characterizations reveal that the MZO-NCs significantly enhance charge extraction from CQD solids and diminish the charge accumulation at the ETL/CQD interface, suppressing charge interfacial recombination. These important results suggest that the low-temperature processed MZO-NCs are very promising for use in efficient flexible solar cells or other flexible optoelectronic devices.
A family of photocatalysts for water splitting into hydrogen was prepared by distributing TiO(6) units in an MTi-layered double hydroxide matrix (M = Ni, Zn, Mg) that displays largely enhanced photocatalytic activity with an H(2)-production rate of 31.4 μmol h(-1) as well as excellent recyclable performance. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) mapping and XPS measurement reveal that a high dispersion of TiO(6) octahedra in the layered doubled hydroxide (LDH) matrix was obtained by the formation of an M(2+)-O-Ti network, rather different from the aggregation state of TiO(6) in the inorganic layered material K(2)Ti(4)O(9). Both transient absorption and photoluminescence spectra demonstrate that the electron-hole recombination process was significantly depressed in the Ti-containing LDH materials relative to bulk Ti oxide, which is attributed to the abundant surface defects that serve as trapping sites for photogenerated electrons verified by positron annihilation and extended X-ray absorption fine structure (EXAFS) techniques. In addition, a theoretical study on the basis of DFT calculations demonstrates that the electronic structure of the TiO(6) units was modified by the adjacent MO(6) octahedron by means of covalent interactions, with a much decreased bandgap of 2.1 eV, which accounts for its superior water-splitting behavior. Therefore, the dispersion strategy for TiO(6) units within a 2D inorganic matrix can be extended to fabricate other oxide or hydroxide catalysts with greatly enhanced performance in photocatalysis and energy conversion.
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